Two-center interference and ellipticity in high-order harmonic generation from H2+_2^+

We present a theoretical investigation into the two-center interference in aligned H$_2^+$. The influence of the laser field on the recombination step is investigated by comparing laser-induced harmonic generation with harmonic generation from field-free collisions of Gaussian wave packets with the core. We find that for different Gaussian wave packets colliding with the molecule, the interference minimum occurs at the same alignment angle. The same result is obtained for the laser-induced spectrum when only a single electronic trajectory per harmonic contributes. When multiple electronic trajectories contribute, we find an effect on the minimum position because the interference between short and long trajectories is alignment-dependent. The two-center interference and the influence of the Coulombic potential are clearly seen not only in the harmonic intensity and phase but also in the polarization direction and ellipticity. We observe significant ellipticity of the emitted radiation around the two-center interference minimum.Comment: 10 pages, 15 figures; v2: clearer figures and other small changes; v3: small correction

Control of recollision wave packets for molecular orbital tomography using short laser pulses

The tomographic imaging of arbitrary molecular orbitals via high-order harmonic generation requires that electrons recollide from one direction only. Within a semi-classical model, we show that extremely short phase-stabilized laser pulses offer control over the momentum distribution of the returning electrons. By adjusting the carrier-envelope phase, recollisions can be forced to occur from mainly one side, while retaining a broad energy spectrum. The signatures of the semi-classical distributions are observed in harmonic spectra obtained by numerical solution of the time-dependent Schr\"{o}dinger equation.Comment: 8 pages, 4 figures; v2: Added some extra clarifications; v3: minor grammatical change

Molecular imaging using high-order harmonic generation and above-threshold ionization

Accurate molecular imaging via high-order harmonic generation relies on comparing the harmonic emission from a molecule and an adequate reference system. However, an ideal reference atom with the same ionization properties as the molecule does not always exist. We show that for suitably designed, very short laser pulses, a one-to-one mapping between high-order harmonic frequencies and electron momenta in above-threshold ionization exists. Comparing molecular and atomic momentum distributions then provides the electron return amplitude in the molecule for every harmonic frequency. We show that the method retrieves the molecular recombination transition moments highly accurately, even with suboptimal reference atoms.Comment: 5 pages, 4 figure

Emission times in high-order harmonic generation

We calculate the emission times of the radiation in high-order harmonic generation using the Gabor transform of numerical data obtained from solving the time-dependent Schrödinger equation in one, two, and three dimensions. Both atomic and molecular systems, including nuclear motion, are investigated. Lewenstein model calculations are used to gauge the performance of the Gabor method. The resulting emission times are compared against the classical simple man's model as well as against the more accurate quantum orbit model based on complex trajectories. The influence of the range of the binding potential (long or short) on the level of agreement is assessed. Our analysis reveals that the short-trajectory harmonics are emitted slightly earlier than predicted by the quantum orbit model. This partially explains recent experimental observations for atoms and molecules. Furthermore, we observe a distinct signature of two-center interference in the emission times for H2 and D2. © 2010 The American Physical Society

Molecular Orbital Tomography using Short Laser Pulses

Recently, a method to image molecular electronic wave functions using high harmonic generation (HHG) was introduced by Itatani \textit{et al.\} [Nature {\textbf{432}}, 876 (2004)]. We show that, while the tomographic reconstruction of general orbitals with arbitrary symmetry cannot be performed with long laser pulses, this becomes possible when extremely short pulses are used. An alternative reconstruction equation based on momentum matrix elements, rather than on dipole matrix elements, is proposed. We present simulations of the procedure for 2D model systems based on numerical solutions of the time-dependent Schr\"{o}dinger equation, and present results from further post-processing of the reconstructed orbitals.Comment: 5 pages, 2 figure

Tomographic imaging of molecular orbitals in length and velocity form

Max-Planck-Institut für Kernphysik, Heidelber